0000000000121757
AUTHOR
Jan Becker
Light-Scattering and -Absorption of Nanoparticles
To understand the optical response of nanoparticles to the incident light, a theoretical description is needed, which is given in this chapter. In a first approximation, these optical properties can be described using a quasi-static model, which assumes a particle-size much smaller than the wavelength of the light. The derivation of the polarizability of a sphere, which describes its optical properties, and further extensions for spheroidal, rod-shaped and coated particles are given in Sect. 2.2.
Protein-membrane interaction probed by single plasmonic nanoparticles.
We present a nanosized and addressable sensor platform based on membrane coated plasmonic particles and show unequivocally the covering with lipid bilayers as well as the subsequent detection of streptavidin binding to biotinylated lipids. The binding is detected on membrane covered gold nanorods by monitoring the spectral shift by fast single particle spectroscopy (fastSPS) on many particles in parallel. Our approach allows for local analysis of protein interaction with biological membranes as a function of the lateral composition of phase separated membranes.
The Optimal Aspect Ratio for Plasmonic Bio-Sensing
The sensitivity of plasmonic particles to the immediate dielectric environment allows to monitor the dielectric constant of liquids and binding events of molecules to the gold particle surface. Here, by means of simulations and experiments, I investigate which aspect ratio (AR) of gold nanorods is ideal for plasmonic sensing by employing various measures for “ideal” behavior.
Improving the Course of Depressive Symptoms After Inpatient Psychotherapy Using Adjunct Web-Based Self-Help: Follow-Up Results of a Randomized Controlled Trial
Background We recently showed in a randomized controlled trial that Web-based self-help as an adjunct improved the effectiveness of multimodal inpatient psychotherapy for depression. Objective The aims of this study were (1) to determine whether a Web-based self-help adjunctive to multimodal inpatient psychotherapeutic treatment could also improve the course of depressive symptoms and (2) to identify predictors of residual depressive symptoms at follow-up. Methods Overall, 229 patients were randomized either to the Web-based self-help intervention group (Deprexis) or an active control group (Web-based information about depression and depressive symptoms) in addition to multimodal inpatient…
Self Calibrating Nano-Ruler
The aim of a nanoruler is to measure distances on a length scale in the order of nanometers. This concept can be realized by two plasmonic nanoparticles (usually spheres), which are placed within a short distance to each other. Since the plasmon modes of both particles are coupled, they influence each other along the interparticle axis (i.e. longitudinal plasmon mode, resulting in a shift of the resonance wavelength compared to the single particle. Because the resulting resonance wavelength depends on the interparticle distance, the spectral investigation of such a dimer allows the determination of the interparticle distance.
Increasing Nanoparticles’ Refractive Index Sensitivity
Since the plasmon resonance of nanoparticles depends on the refractive index of the immediate environment, these particles form the basis of many sensing schemes . The sensitivity of plasmon sensors for the detection of changes in the environment varies greatly and depends on the particle material and its morphology (size and shape). To further increase this sensitivity by chemical modifications was another goal of my work.
Mapping the polarization pattern of plasmon modes reveals nanoparticle symmetry.
We study the wavelength and polarization dependent plasmon resonances of single silver and gold nanorods, triangles, cubes, and dimers with a novel single particle spectroscopy method (RotPOL). In RotPOL, a rotating wedge-shaped polarizer encodes the full polarization information of each particle within one image. This reveals the symmetry of the particles and their plasmon modes, allows analyzing inhomogeneous samples and the monitoring of particle shape changes during growth in situ.
Highly Sensitive plasmonic silver nanorods
We compare the single-particle plasmonic sensitivity of silver and gold nanorods with similar resonance wavelengths by monitoring the plasmon resonance shift upon changing the environment from water to 12.5% sucrose solution. We find that silver nanoparticles have 1.2 to 2 times higher sensitivity than gold, in good agreement with simulations based on the boundary-elements-method (BEM). To exclude the effect of particle volume on sensitivity, we test gold rods with increasing particle width at a given resonance wavelength. Using the Drude-model of optical properties of metals together with the quasi-static approximation (QSA) for localized surface plasmons, we show that the dominant contrib…
Plasmonic Focusing Reduces Ensemble Linewidth of Silver-Coated Gold Nanorods
Silver coating gold nanorods reduces the ensemble plasmon line width by changing the relation connecting particle shape and plasmon resonance wavelength. This change, we term "plasmonic focusing", leads to less variation of resonance wavelengths for the same particle size distribution. We also find smaller single particle linewidth comparing resonances at the same wavelength but show that this does not contribute to the ensemble linewidth narrowing.
Plasmonic-photonic hybrid cavity for tailored light-matter coupling
We propose and demonstrate a hybrid cavity system in which metal nanoparticles are evanescently coupled to a dielectric photonic crystal cavity using a nanoassembly method. While the metal constituents lead to strongly localized fields, optical feedback is provided by the surrounding photonic crystal structure. The combined effect of plasmonic field enhancement and high quality factor (Q ≈ 900) opens new routes for the control of light-matter interaction at the nanoscale.
Nanoassembled plasmonic-photonic hybrid cavity for tailored light-matter coupling.
We propose and demonstrate a hybrid cavity system in which metal nanoparticles are evanescently coupled to a dielectric photonic crystal cavity using a nanoassembly method. While the metal constituents lead to strongly localized fields, optical feedback is provided by the surrounding photonic crystal structure. The combined effect of plasmonic field enhancement and high quality factor (Q approximately 900) opens new routes for the control of light-matter interaction at the nanoscale.
Online Self-Help as an Add-On to Inpatient Psychotherapy: Efficacy of a New Blended Treatment Approach.
<b><i>Background:</i></b> Depression is one of the most frequent and costly mental disorders. While there is increasing evidence for the efficacy of online self-help to improve depression or prevent relapse, there is little evidence in blended care settings, especially combined with inpatient face-to-face psychotherapy. Therefore, we evaluated whether an evidence-based online self-help program improves the efficacy of inpatient psychotherapy. <b><i>Methods:</i></b> A total of 229 depressed patients were randomly allocated either to an online self-help program (intervention group [IG]; Deprexis) or an active control group (CG; weekly online inf…
Plasmonic Core–Satellite Assemblies as Highly Sensitive Refractive Index Sensors
Highly sensitive and spectrally tunable plasmonic nanostructures are of great demand for applications such as SERS and parallel biosensing. However, there is a lack of such nanostructures for the midvisible spectral regions as most available chemically stable nanostructures offer high sensitivity in the red to far red spectrum. In this work, we report the assembly of highly sensitive nanoparticle structures using a hydroxylamine mediated core–satellite assembly of 20 nm gold nanoparticle satellites onto 60 nm spherical gold cores. The average number of satellites allows tuning the plasmon resonance wavelength from 543 to 575 nm. The core–satellite nanostructures are stable in pH ranges from…
Single Gold Nanoparticle Growth Monitored in situ
The novel fastSPS setup is used to study the growth process of rodshaped gold nanoparticles in the presence of surfactant molecules. It is observed that the particles grow mainly in the direction of the short rod axis, resulting in a decrease of the aspect ratio. This is, to the best of my knowledge, the first real-time optical observation of nanoparticle growth on a single-particle level (results were published in reference ). In collaboration with Olaf Schubert the nanoparticle growth was also monitored using the novel RotPOL setup. Here a decrease of the average polarization anisotropy \(PA\) is observed.
Protein-Membrane Interaction
In the following chapter I present a nanosized and addressable protein sensor platform based on membrane coated plasmonic particles. I show unequivocally the covering of gold nanorods with lipid bilayers and thereafter the subsequent detection of streptavidin binding to biotin moities in the lipids. The binding of the streptavidin on the membrane covered gold nanorods is detected by monitoring the spectral shift by fast single particle spectroscopy (fastSPS) on many particles in parallel.
Au@MnO-“Nanoblumen” - Hybrid-Nanokomposite zur selektiven dualen Funktionalisierung und Bildgebung
In j ngster Vergangenheit hat das Interesse f r die Entwicklung von Hybrid-Nanostrukturen, die sich aus verschiedenen Materialien zusammensetzen, in erheblichem Mase zugenommen. Es wurde berichtet, dass die Zusammenf hrung verschiedener Nanomaterialien, die ihrerseits spezifische optische, magnetische oder elektronische Eigenschaften aufweisen, zu Kompositen aus mehreren dieser Komponenten, deren individuelle Eigenschaften ver ndern oder sogar verbessern k nnen. Durch gezielte Optimierung der Struktur und der Grenzfl chenwechselwirkung innerhalb der Nanokomposite k nnte eine breite Basis f r zuk nftige Technologien geschaffen werden, beispielweise f r die synchrone Biomarkierung, Proteintre…
Plasmonic Focusing Reduces Ensemble Linewidth
In this chapter I present an effect the coating of gold nanorods with a silver shell is evocating: a reduction of the ensemble plasmon linewidth by changing the plasmon-shape relation, which connects the particle shape with its plasmon resonance wavelength. This change, we term “plasmonic focusing” (Sect. 10.2), leads to less variation of resonance wavelengths for the same particle size distribution. Section 10.3 explains the effect of increasing single particle linewidth during the coating process, which is therefore not the reason for the observed ensemble linewidth decrease. This is rather a result from a change in the plasmon-shape relation explained in Sect. 10.4. Using a simple model,…
Synthesis of Nanoparticles
In this chapter I describe the synthetic methods for the particles used in this work. Initially bare gold nanorods are synthesized , which are used to investigate continuously the growth of bigger nanoparticles and the protein-membrane interaction on a single particle level . To reduce the single particle linewidth and therefore to increase the sensitivity on changes in the refractive index , these rods are coated with a thin silver shell . Another method to increase the sensitivity of nanoparticles is to produce hollow rod-shaped nanorattles, which were synthesized by Yuriy Khalavka . To investigate the polarization depend scattering spectra of different shapes with the RotPOL setup , diff…
Synthesis of rod-shaped gold nanorattles with improved plasmon sensitivity and catalytic activity.
We prepared rod-shaped gold nanorattles solid gold nanorods surrounded by a thin gold shell using a galvanic replacement process starting with silver-coated gold nanorods. These structures are very promising candidates for catalytic applications and optimized plasmon sensors. They combine the advantages of rods (low plasmon resonance frequency, large polarizability, small damping) with the high surface area of hollow structures. The plasmon sensitivity to changes in the dielectric environment is up to 50% higher for gold nanorattles compared to gold nanorods with the same resonance frequency and 6x higher than for plasmons in spherical gold nanoparticles. The catalytic activity measured for…
Au@MnO nanoflowers: hybrid nanocomposites for selective dual functionalization and imaging.
Recently, the development of hybrid nanostructures consisting of various materials has attracted considerable interest. The assembly of different nanomaterials with specific optical, magnetic, or electronic properties to multicomponent composites can change and even enhance the properties of the individual constituents. Specifically tuning the structure and interface interactions within the nanocomposites has resulted in novel platforms of materials that may lead the way to various future technologies, such as synchronous biolabeling, protein separation and detection, heterogeneous catalysis, and multimodal imaging in biomedicine. Of the various kinds of nanomaterials, gold nanorods show an…
Gold Nanoparticle Growth Monitored in situ Using a Novel Fast Optical Single-Particle Spectroscopy Method
Size- and shape-dependent optical properties of gold nanorods allow monitoring their growth using a novel fast single-particle spectroscopy (fastSPS) method. FastSPS uses a spatially addressable electronic shutter based on a liquid crystal device to investigate particles randomly deposited on a substrate, orders of magnitude faster than other techniques. We use fastSPS to observe nanoparticle growth in situ on a single-particle level and extract quantitative data on nanoparticle growth.
Plasmonic Silver Nanorod Sensitivity: Experiment and Simple Theoretical Treatment
We compare the plasmonic sensitivity of silver and gold nanorods with similar resonance wavelengths by monitoring the plasmon resonance shift of single noble metal nanorods upon changing the environment from water to sucrose solution. We find that silver nanorods have 1.2 to 2 times higher sensitivity than gold in good agreement with simulations based on the boundary-elements-method (BEM). To exclude the effect of particle volume on sensitivity, we test gold rods with increasing particle width at a given resonance wavelength. Using the Drude-model of optical properties of metal together with the quasi-static approximation (QSA) for localized surface plas-mons, we show that the dominant cont…